With wearable electronics rapidly coming into fashion, research into flexible energy storage devices and in particular, pliable electrodes, is attracting a lot of attention. Pliable electrodes are usually fabricated by intercalating an active material in a flexible matrix with superior mechano‐electrical properties, and can be grouped either as substrate‐supported or free‐standing. Depending on their mode of deformation the electrodes can be labeled as bendable, compressible or stretchable. Recent progress and challenges in the design and fabrication of pliable electrodes for constructing flexible lithium ion batteries and flexible supercapacitors are highlighted. 2 pliable core‐shell structure electrodes fabricated from: a) carbon nanotube sponge embedded with MoS₂ nanoparticles and b) electrospun polyethylene terephthalate fibers impregnated with graphene nanoplatelets are also presented.

Harnessing random micromeso-scale ambient energy is not only clean and sustainable, but it also enables self-powered sensors and devices to be realized. Here we report a robust and self-powered kinematic vector sensor fabricated using highly pliable organic films that can be bent to spread over curved and uneven surfaces. The device derives its operational energy from a close-proximity triboelectrification of two surfaces: a polytetrafluoroethylene film coated with a two-column array of copper electrodes that constitutes the mover and a polyimide film with the top and bottom surfaces coated with a two-column aligned array of copper electrodes that comprises the stator. During relative reciprocations, the electrodes in the mover generate electric signals of ±5 V to attain a peak power density of ≥65 mW m⁻²at a speed of 0.3 ms⁻¹. From our 86,000 sliding motion tests of kinematic measurements, the sensor exhibits excellent stability, repeatability and strong signal durability.

3D electrode design is normally opted for multiple advantages, however, instability/detachment of active material causes the pulverization and degradation of the structure, and ultimately poor cyclic stability. Here, a dually protected, highly compressible, and freestanding anode is presented for sodium‐ion batteries, where 3D carbon nanotube (CNT) sponge is decorated with homogeneously dispersed CoSe₂ nanoparticles (NPs) which are protected under carbon overcoat (CNT/CoSe₂/C). The 3D CNT sponge delivers enough space for high mass loading while providing high mechanical strength and faster conduction pathway among the NPs. The outer amorphous carbon overcoat controls the formation of solid electrolyte interphase film by avoiding direct contact of CoSe₂ with electrolyte, accommodates large volume changes, and ultimately enhances the overall conductivity of cell and assists in transmitting electron to an external circuit. Moreover, the hybrid can be densified up to 11‐fold without affecting its microstructure that results in ultrahigh areal mass loading of 17.4 mg cm⁻² and an areal capacity of 7.03 mAh cm⁻² along with a high gravimetric capacity of 531 mAh g⁻¹ at 100 mA g⁻¹. Thus, compact and smart devices can be realized by this new electrode design for heavy‐duty commercial applications.